Magnesium-ion batteries (MIBs) have great potential in large-scale energy storage field with high capacity, excellent safety, and low cost. However, the strong solvation effect of Mg will lead to the formation of solvated ions in electrolytes with larger size and sluggish diffusion/reaction kinetics. Here, the concept of interfacial catalytic bond breaking is first introduced into the cathode design of MIBs by hybriding MoS quantum dots with VS (VS@MQDs) as the cathode. The "in situ dynamic catalysis and re-equilibration" effects can catalyze the Cl-Mg bond breaking and trigger single Mg insertion/extraction chemistries, which can significantly accelerate the diffusion and reaction kinetics, as verified by the decreased diffusion energy barriers (0.26 eV for Mg vs 2.47 eV for MgCl) and fast diffusion coefficient. Benefitting from these dynamic catalysis effects, the constructed VS@MQD-based MIBs deliver a high discharge capacity of ∼120 mA h g at 200 mA g and a long-term cyclic stability of 1000 cycles at 1 A g. The improved performance and detailed characterizations well prove that the active ions in MIBs change from MgCl/MgCl to Mg with fast kinetics.
Download full-text PDF |
Source |
---|---|
http://dx.doi.org/10.1021/acsami.3c03097 | DOI Listing |
Angew Chem Int Ed Engl
January 2025
University of Basel, Department of Chemistry, St. Johanns-Ring 19, 4056, Basel, SWITZERLAND.
Despite the growing importance of planar chiral macrocyclophanes owing to their unique properties in different areas of chemistry, methods that are effective in controlling their planar chirality are restricted to certain molecular scaffolds. Herein, we report the first Pd(0)-catalyzed enantioselective intermolecular C-H arylation that induces planar chirality by installing bulky aryl groups through dynamic kinetic resolution (DKR). A computer-assisted approach allowed a fine-tuning of the structure of the employed chiral bifunctional phosphine-carboxylate ligands to achieve high enantioselectivities.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
CNRS/UCSD, Chemistry, University of California, San Diego, 5213 Pacific Hall,, Department of Chemistry, 92093-0343, La jolla, UNITED STATES.
N-Heterocyclic carbene (NHC) ligands possess the ability to stabilize metal-based nanomaterials for a broad range of applications. With respect to metal-hydride nanomaterials, however, carbenes are rare, which is surprising if one considers the importance of metal-hydride bonds across the chemical sciences. In this study, we introduce a bottom-up approach leveraging preexisting metal-metal m-center-n-electron (mc-ne) bonds to access a highly stable cyclic(alkyl)amino carbene (CAAC) copper-hydride nanocluster, [(CAAC)6Cu14H12][OTf]2 with superior stability compared to Stryker's reagent, a popular commercial phosphine-based copper hydride catalyst.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
State Key Laboratory of Bioreactor Engineering, East China University of Science and Technology, Shanghai 200237, China.
Taming highly enolizable aldehydes for catalytic asymmetric C-C coupling with nucleophiles remains an elusive challenge compared to widely explored simple alkyl or aryl aldehydes. Herein, we use ThDP-dependent enzymes to realize the direct C-C coupling of highly enolizable 2-phosphonate aldehydes with in situ-generated dynamically reversible nucleophiles (acyl anions). Unlike NHC-mediated reactions that yield complex mixtures of multiple adducts, our enzymatic process selectively produces biologically active β-hydroxy phosphonates with high yields (up to 95%) and excellent enantioselectivities (up to 99% ee).
View Article and Find Full Text PDFACS Nano
January 2025
School of Materials Science and Engineering, China University of Petroleum (East China), Qingdao 266580, Shandong, China.
Core-shell structures demonstrate superior capability in customizing properties across multiple scales, offering valuable potential in catalysis, medicine, and performance materials. Integrating functional nanoparticles in a spatially controlled manner is particularly appealing for developing sophisticated architectures that support heterogeneous characteristics and tandem reactions. However, creating such complex structures with site-specific features remains challenging due to the dynamic microenvironment during the shell-forming process, which considerably impacts colloidal particle assembly.
View Article and Find Full Text PDFChem Rev
January 2025
Beijing National Laboratory for Molecular Science, New Cornerstone Science Laboratory, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, People's Republic of China.
Heterogeneous catalysts are pivotal to the chemical and energy industries, which are central to a multitude of industrial processes. Large-scale industrial catalytic processes rely on special structures at the nano- or atomic level, where reactions proceed on the so-called active sites of heterogeneous catalysts. The complexity of these catalysts and active sites often lies in the interfacial regions where different components in the catalysts come into contact.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!